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Applied Water Science

, 8:128 | Cite as

Groundwater arsenic contamination and their variations on episode of drought: Ter River delta in Catalonia, Spain

  • René Ventura-HouleEmail author
  • Xavier Font
  • Lorenzo Heyer
Open Access
Short Research Communication
  • 570 Downloads

Abstract

The analysis and prospection using hydrogeochemical methodologies on arsenic (As) contamination episode in region of Spain (Girona, Cataluña) was investigated on the period (2000–2011), to analyze the mechanisms and characteristics of process on the solubilization of As in groundwater and effects of the episode of severe drought (2006–2007) on hydrogeochemical characteristics of the aquifer. The aquifer of study is a Mediterranean Delta; the geology of the zone has influence from sedimentary deposition of Ter River Basin and the prograde and draw back of the history coastline. The aquifer is an alluvial system where mean concentration of (As) is 30 µg/L in groundwater; parallel to this, the concentrations of elements iron (Fe) and manganese (Mn) exceed the guidelines of the World Health Organization (Guidelines for drinking-water quality electronic resource incorporating 1st and 2nd addenda, vol 1, Recommendations, 3rd edn, World Health Organization, Geneva, 2006) for drinking water. Range concentrations from other elements found in the groundwater were: Aluminum (Al, 4–716 µg/L), Barium (Ba, 48–603 µg/L), Cupper (Cu, 0.2–105.3 µg/L), Chrome (Cr, 1.1–47 µg/L) and Nickel (Ni, 1–51 µg/L). The arsenic solubilization trigger mechanism comes from desorption of oxide minerals and reduction related on neutral pH and reductive environment; the source of this kind of oxides is probably from marine sediments deposited in the process of delta’s formation. During the climatic event of drought (2006–2007), the As concentration was responding to decline levels of the water volume on the aquifer, increasing their concentration and localized in a small area of the study zone, and these are effects of the reduction in groundwater flow on the aquifer.

Keywords

Arsenic Aquifer Sedimentary basin Drought 

Introduction

The adverse effects in humans, caused by intake of arsenic (As) in diet elements, are a worldwide serious scope for the human health protection. Arsenic (As) is recognized as one of the most serious inorganic contaminants in drinking water in the world, particularly in regions where the concentration of arsenic in groundwater supplies is naturally high (Smedley and Kinniburgh 2002). Many areas around the world have problems with contamination related to human activities like mining and smelting activities, coal combustion, tanning waste, pigment production, wood conservation, increased growth in feedlot-raised poultry and use of pesticides (Gomez et al. 2009; Pérez-Carrera and Fernández 2010). The contamination with As caused by human activities generally is localized and in almost all cases is not a health risk. Otherwise, natural pollution is present in regions with geological formations rich in arsenic, as plutonic rocks and sedimentary basins, used to occupy large geographical areas where water sources are compromised by the migration of arsenic aqueous forms to groundwater (Smedley and Kinniburgh 2002). This causes serious problems, for the water supply systems, and increases the population at risk (Anawar et al. 2006; Devi et al. 2010).

The process of (As) mobilization from aquifer substrate materials is regulated by hydrogeochemical process where the presence of oxidized and/or reduced mineral phases and the cofactors are associated with arsenic-rich solid phases. Arsenic-rich aquifers are characterized by elevated concentrations of dissolved iron, bicarbonate, ammonium ion and phosphate under reducing conditions and neutral pH (Anawar et al. 2006; Gomez et al. 2009; Hernandez-Garcia and Custodio 2004).

The species of (As) found in the environment are arsenic(III) and arsenic(V); the predominant species is determined by pH and reduction/oxidation potential. In many aquatic environments (As) species are in the form of oxyacid. Under oxidizing conditions (As), species are in the form of arsenic (V) or arsenate anions (AsO43−), where (H2AsO4) is the most thermodynamically stable species at pH between 2 and 7 (Ryzhenko et al. 2009). In contrast, under reducing conditions the predominant species are As(III) or arsenite anions (AsO33−), where neutral arsenite (H3AsO3) is thermodynamically the most stable species up to about pH 9 (Krainov et al. 2007; Ryzhenko et al. 2009). Arsenates, arsenate anions, and neutral arsenite constitute the main targets for field analysis, and they are actors in groundwater natural pollution (Pérez-Carrera and Fernández 2010).

The hydrogeochemical mechanisms for desorption of arsenic from the mineral pyrite are defined for the relationship of As with sulfate and iron. When the sulfide oxidation is the dominant process of the passing of As to its aqueous forms, a positive correlation can be found between the concentrations of (SO42−) and (As) (Smedley and Kinniburgh 2002). In the sedimentary basins where the groundwater has a neutral pH and reducing environment associated with the presence of fresh organic matter, the geochemical environment is a determining factor for the solubility of arsenic (Selim et al. 2010). The basic trigger mechanism for the dissolution of As in porewaters environments of sedimentary basins, with neutral pH and reducing geochemical environments, can be associated to reduction-related dissolution of Fe and Mn oxides minerals, which results in the migration of As(III), Fe(II) and Mn(II) into the aqueous phase where they can reach high concentrations of these elements with a positive correlation between them (Smedley and Kinniburgh 2002), while the concentrations of (SO42−) remains low (less than 1 mg/L). The high concentrations of phosphates, bicarbonates, silicates, and, possibly, organic matter may be favorable for As desorption (Anawar et al. 2006; Ryzhenko et al. 2009).

Of the regions of the world with groundwater arsenic problems, the worse emblematic episodes are localized on sedimentary basins (Smedley and Kinniburgh 2002). The iconic case of quaternary alluvial and deltaic sediment is associated with the Ganges–Brahmaputra–Meghna river system in Bangladesh, where more than 35 million people must drink groundwater containing (As) at concentrations greater than 50 µg/L (Chakraborti et al. 2015). Other examples are the porewater from the Kalix River estuary of northern Sweden with concentrations in the range 1.3–166 µg/L and porewater from clay sediments of Saskatchewan, Canada, where As was found at concentrations in the range 3.2–99 µg/L (Wang and Mulligan 2005; Rahman et al. 2007).

The scope of this work is to analyze the origin and the trigger mechanism on solubilization of (As) in aquifer of Ter River delta. Associated with the identification of these processes, it is possible to see the effects of the drought period on the hydrogeochemical mechanisms and on the water quality of the aquifer studied.

Materials and methods

This research was realized analyzing information collected by the Agencia Catalana del Agua (ACA) through the monitoring program denominated “Register and Control of Quality of Waterbodies in Catalonia.” This is a 10-year (2000–2010) database with annual records of the concentration level of arsenic in the Ter River delta, and other aquifers of Catalonia, Spain, also includes the next water characterization parameters: electrical conductivity (EC), reduction–oxidation potential (REDOX), hydrogen potential (pH), temperature (T), major ions (SO42−, Cl, HCO31−, Ca2+, Mg2+, Na+), and trace elements presences (As, Ba, Co, Cu, Cr, Sr, Fe). The sampling periodicity of the monitoring program was annual, generally effectuated in the period winter-spring on wells with different kind of uses basically a mix of municipal sources of water for human supply and private property wells used basically for agricultural camps of rice and fruit trees. The chemical analyses are made in certificated institutional laboratories.

To validate the information presented in the database, the Geochemistry, Petrology and Geological Prospecting Department of the Universitat de Barcelona (UB) in the year (2011), realized a sampling program, following the same protocol of ACA. The samples were sent to ACTLabs laboratories in Canada for its analysis on high-resolution inductively coupled plasma mass spectrometry (ICP-MS). The results reported by the ACA on 2011 were compared with the results of the UB sampling, and no significant difference was found between them.

Geographical and hydrogeochemical setting

The studied zone is localized in a rural activities territory of the state of Catalonia in the northeast of Spain (Fig. 1); it extends through the municipals demarcations of Gualta, Torroella de Mongrí, Palau Sator and Ullastret. The area is Ter River delta well known as Baix Emporda basin, an ecohydrology region formed for outfall delta in the Mediterranean coast. This delta has a quaternary sedimentary origin, which was developed as result of trailing sediments from Ter and Daró rivers through the historical process of interaction advance and retraction during the evolution of the coastline. This Delta is the end of a Ter River delta system with approximate 3010 km2 area with a mean of rain of 740 mm per year. The groundwater delta system is formed for different permeability units layered sediments with mean 2772 Hm3 of capacity for water storage (Montaner and Subiranas 2009).
Fig. 1

Baix Emporda, Ter River delta map showing the sampling sites

Drought episode

During first decade of 2000, the area of Catalonia suffers an episode of pluviometric drought, which affected an enormous region of Europe. In this climatic event, the water sources of human supply technically were exhausted and provoke a serious restriction and extraordinary measures for all waters uses. In the period of 2005–2008, the water deficit was over 80% (Fig. 2) (Altava-Ortiz et al. 2017); due to consecutive years in rain deficit in April of the 2007, the authorities declare the emergency state for drought (Diario Oficial de la Generalitat de Catalunya, Decreto 257/2007). This situation continued through all 2007 without rain and the deficit grew almost to 90%. Until May of 2008, the situation was very difficult, the reserves of water a regional level was empty, and the emergency was alleviating in July month when it starts to rain and continues the next months. In January 2009 the emergency of drought was declared finished by the authorities (Agencia Catalana del Agua 2009).
Fig. 2

Water deficit temporal evolution period years 1998–2015

Source: Reproduced with permission from Altava-Ortiz et al. (2017)

Results and discussion

On the study area, the concentration of As does not exceed the maximum limit recommended for the drinking water proposed for the WHO of 10 µg/L (WHO 2006), except for a small area of 6 km2, where the As concentration ranges from 20 to 90 µg/L (Fig. 3). Through the 10 years of observation, the concentration levels of As remain constant particularly in this zone. The general groundwater analysis (Table 1) presents metals which have sanitary important considerations, like Fe, Mn, Al, Ba and others.
Fig. 3

Arsenic concentrations in periods

Table 1

Database of parameters from waters collected in the study area

Site

Year

E.C.

pH

Eh

HCO3

SO42−

Cl

Ca2+

Mg2+

Na+

Al

As

Ba

Co

Cu

Cr

Fe

Mn

Mo

Ni

Pb

µS/cm

mV

mg/L

mg/L

mg/L

mg/L

mg/L

mg/L

µg/L

µg/L

µg/L

µg/L

µg/L

µg/L

µg/L

µg/L

µg/L

µg/L

µg/L

3

2002

1178

7.8

N.N.

318

158

99

135

64

55

n.d.

n.d.

122

n.d.

n.d.

n.d.

178

941

n.d.

n.d.

n.d.

4

2002

12,468

N.N.

67

623

593

6803

407

3495

3495

n.d.

n.d.

234

3

14

n.d.

1105

2931

2

n.d.

n.d.

9

2002

1536

N.N.

176

467

230

155

185

61

98

62

n.d.

166

3

n.d.

n.d.

2091

945

n.d.

n.d.

13

13

2002

1666

N.N.

220

651

128

170

171

97

115

61

n.d.

82

3

n.d.

n.d.

4400

1211

n.d.

n.d.

n.d.

14

2002

1519

N.N.

216

587

167

178

180

114

63

72

n.d.

93

1

8

n.d.

1495

576

n.d.

n.d.

n.d.

17

2002

1032

N.N.

352

353

175

112

160

54

64

80

16

145

2

4

n.d.

2013

831

1

n.d.

n.d.

23

2005

873

N.N.

137

493

220

132

200

73

47

n.d.

6

239

n.d.

86

n.d.

1562

312

n.d.

43

n.d.

1

2005

878

N.N.

157

401

195

116

172

67

51

n.d.

n.d.

153

n.d.

n.d.

n.d.

831

408

n.d.

n.d.

n.d.

4

2005

18,250

N.N.

72

553

207

6611

180

4863

4199

n.d.

n.d.

207

n.d.

19

n.d.

11,250

4921

n.d.

n.d.

11

9

2005

1496

7.4

N.N.

534

134

109

141

91

112

n.d.

n.d.

123

n.d.

n.d.

n.d.

889

941

n.d.

n.d.

n.d.

13

2005

1194

7.3

N.N.

377

84

89.5

135

51

91

n.d.

n.d.

67

n.d.

n.d.

n.d.

223

1268

n.d.

n.d.

n.d.

14

2005

1387

7.4

N.N.

567

855

7243

420

4199

70

n.d.

n.d.

98

n.d.

n.d.

n.d.

361

703

n.d.

n.d.

n.d.

17

2005

768

N.N.

222

359

56

75.7

106

43

44

n.d.

88

106

n.d.

n.d.

n.d.

354

1172

n.d.

n.d.

n.d.

1

2007

932

7.2

N.N.

396

110

85

156

54

54

n.d.

n.d.

140

n.d.

11

n.d.

n.d.

n.d.

12

n.d.

n.d.

4

2007

14859

7

N.N.

593

957

6194

281

376

3888

n.d.

n.d.

130

n.d.

n.d.

n.d.

n.d.

3968

n.d.

n.d.

n.d.

9

2007

1040

7.3

N.N.

219

109

61

96

45

74

n.d.

n.d.

48

n.d.

n.d.

n.d.

262

888

n.d.

n.d.

n.d.

14

2007

N.N.

N.N.

N.N.

470

336

158.5

228

100

73

n.d.

n.d.

109

n.d.

n.d.

n.d.

1485

601

n.d.

n.d.

n.d.

17

2007

922

7.4

N.N.

440

98

76

138

541

54

n.d.

72

189

n.d.

n.d.

n.d.

1410

1485

n.d.

n.d.

n.d.

20

2007

793

7

N.N.

458

133

68.2

125

45

38

n.d.

n.d.

53

n.d.

n.d.

n.d.

n.d.

n.d.

n.d.

n.d.

n.d.

22

2007

998

7.7

N.N.

405

69

43.1

140

37

46

n.d.

n.d.

72

n.d.

10

n.d.

n.d.

n.d.

n.d.

n.d.

n.d.

1

2008

907

7.5

N.N.

744

106

7386

439

1000

50

40

n.d.

139

n.d.

24

n.d.

297

14

n.d.

1

1

10

2008

17,807

N.N.

N.N.

744

1033

7387

439

400

1007

716

n.d.

135

n.d.

n.d.

n.d.

n.d.

5926

n.d.

n.d.

n.d.

14

2008

N.N.

N.N.

N.N.

500

308

207.4

232

107

96

13

4

112

n.d.

8

n.d.

806

577

n.d.

3

n.d.

17

2008

900

7.4

N.N.

363

57

64.7

109

41

54

24

102

134

n.d.

2

n.d.

616

1302

2

1

n.d.

20

2008

827

7.1

N.N.

404

47

62.2

115

53

41

10

n.d.

55

n.d.

1

n.d.

n.d.

n.d.

n.d.

1

n.d.

22

2008

778

7.5

N.N.

370

91

79

141

50

42

17

n.d.

146

n.d.

6

47

n.d.

3

n.d.

n.d.

n.d.

23

2008

977

7.4

N.N.

455

224

457

248

101

135

19

21

603

n.d.

16

n.d.

10,400

791

3

1

2

1

2010

976

N.N.

N.N.

764

102

7867

459

1000

51

n.d.

n.d.

147

n.d.

21

n.d.

n.d.

n.d.

n.d.

1

n.d.

10

2010

24,100

N.N.

N.N.

504

567

7154

413

5395

3125

n.d.

2

157

n.d.

16

n.d.

n.d.

500

2

5

n.d.

14

2010

1476

N.N.

N.N.

374

89

83.7

145

50

91

n.d.

1

86

n.d.

2

n.d.

n.d.

267

n.d.

2

n.d.

17

2010

1051

N.N.

N.N.

442

226

138.9

190

85

52

n.d.

23

143

n.d.

3

n.d.

n.d.

500

1

5

n.d.

20

2010

807

7.1

N.N.

393

118

69.5

129

51

42

n.d.

n.d.

62

n.d.

23

n.d.

n.d.

8

n.d.

n.d.

n.d.

22

2010

602

N.N.

N.N.

403

67

45.8

139

41

42

n.d.

n.d.

135

n.d.

n.d.

n.d.

n.d.

n.d.

n.d.

11

n.d.

23

2010

959

7.7

N.N.

380

95

1106

124

81

81

n.d.

3

231

n.d.

n.d.

n.d.

n.d.

249

1

n.d.

n.d.

1

2011

640

8

40

380

88

85

146

18

52

n.d.

0

223

n.d.

1

n.d.

400

16

n.d.

2

0

4

2011

23,496

7

− 93

763

1028

7865

460

4011

3567

n.d.

58

185

3

54

33

180

6960

4

16

1

17

2011

781

7

− 100

391

117

65

128

19

n.d.

n.d.

n.d.

123

n.d.

3

3

60

1840

1

2

0

20

2011

627

7

127

402

69

44

142

15

43

4

1

55

n.d.

6

n.d.

210

n.d.

1

1

1

22

2011

772

7

84

340

67

63

138

21

40

544

1

151

n.d.

0

n.d.

n.d.

139

n.d.

2

0

23

2011

5590

8

154

475

245

145

200

32

91

n.d.

8

112

n.d.

n.d.

1

60

134

1

7

0

N.N. Not evaluated, n.d. not detected

The groundwater in this area is rich in calcium hydrogen carbonate (CaHCO3) with evolution to (Cl–Na) (Fig. 4). The (Cl–Na) waters present a high EC values (650–20,000 µS/cm) because of marine intrusion, affected for the proximity of the line of coast (Fig. 3). In zones next to coast, the marine intrusion can affect the concentrations of As, by dilution or ion exchange process that can reduce the As presence (Fig. 1) (Smedley and Kinniburgh 2002).
Fig. 4

Evolution of saturation index model of arsenic species in high concentration zones

Trace elements

The presence of elements as (Fe), (Mn) and (Cu) (Table 1) is associated with As in sedimentary basins (Mor et al. 2006); they share hydrogeochemical mechanism of solubilization (Smedley and Kinniburgh 2002). These elements, particularly (Fe) and (Mn), are not correlated to the As concentration (Table 2), but its abundant presence is associated with high concentration of As in the area. Al and Ni showed high variation in area and time, and in some cases, they were above the WHO guidelines (2006). In this study was not found any relation between these elements and As as has been demonstrated by Puthiyasekar et al. (2010).
Table 2

Correlations between most elements present in groundwater of study area

 

HCO 3

SO 4 2

Cl

Ca2+

Mg2+

Na+

As

Ba

Cu

Fe

Mn

HCO 3

1

          

SO 4 2

0.386

1

         

Cl

0.512

0.687

1

        

Ca2+

0.603

0.656

0.846

1

       

Mg2+

0.525

0.752

0.972

0.849

1

      

Na+

0.237

0.815

0.696

0.599

0.718

1

     

As

− 0.246

− 0.191

− 0.131

− 0.223

− 0.129

− 0.112

1

    

Ba

0.141

0.111

0.227

0.207

0.308

0.253

0.069

1

   

Cu

0.175

0.035

0.078

0.015

0.108

0.046

− 0.36

0.265

1

  

Fe

0.147

0.425

0.363

0.256

0.408

0.489

− 0.049

0.277

0.159

1

 

Mn

0.454

0.72

0.842

0.742

0.834

0.682

0.03

0.067

− 0.067

0.29

1

Arsenic relationships and variations

The arsenic does not present statistic correlation with SO42− or other majority ions, which indicates that the origin of As is not come from pyrite or arsenopyrites minerals sources associate with natural rich formations and mine activities (Table 2) (Smedley and Kinniburgh 2002). The low correlation values (zeros and negative) obtained between As and other ions in Table 2 show that it is not associated with these elements. This further supports the position that they exist in the form of oxides, which are solubilized in groundwater.

The neutral pH and the reductive conditions are in accordant situations, where desorption of oxide minerals and reduction-related dissolution of Fe and Mn oxides are the solubility mechanisms of (As) (Ryzhenko et al. 2009; Krainov et al. 2007). These conditions are common in aquifers systems like Baix Ter, with young quaternary sediments, mineral carbonate abundance rich in iron and manganese oxides, low gradient and semiarid environments (Smedley and Kinniburgh 2002; Krainov et al. 2007).

The speciation characterization (Fig. 4), made on a computer program for simulating chemical reactions and transport processes called PHREEQC (pH-Redox-Equilibrium-Concentrations) from the U.S. Geological Service, confirms explanation of mechanism desorption of oxide minerals, given that almost all elements (Fe, As, Mn, Cu and Pb) are in the oxide form. The As are in As(V) and As(III) species which are in negative saturation index, whereby solubilize in elemental forms, the same behavior happens for all other trace elements analyzed; oxides of (Fe, Mn, Cu and Pb) are solubilized in the groundwater with different intensities (Ryzhenko et al. 2009).

Another important clue to support the previous hypothesis is the geologic characteristics and morphology of Baix Emporda aquifer; the delta is an area where sea and land coexist, this aquifer is formed by a big number of deposit of different size materials; the origin of (As) could be a deposit of sediments rich in iron and manganese oxides from antic marine deposits (prehistoric wetlands) which now are part of the aquifer (Montaner and Subiranas 2009; Mondal et al. 2010). The increase in arsenic associates to site 17, because the well is drawing water from a specific deposit of sediments rich in arsenic oxides, as are explained for Montaner and Subiranas (2009) on the study of morphology of the Baix Emporda aquifer. This area situated around the site 17 represents the more affected area on the concentration of arsenic, in year 2008.

Drought effects in groundwater

The concentration of the majority ions was increased on the drought season declared by the authorities, basically caused by progression of the marine intrusion that affects more sampling wells (Fig. 3). The geochemistry milliequivalents analysis showed no variation between seasons (pre-drought, drought, post-drought). Basically, water facie (Ca-HCO3) was constant in areas without marine intrusion affectation.

Elements (Al, As, Mn, Fe and Cr) increase their concentrations in period of drought, this behavior are common with drawdown volumes of water in the aquifer (Gonçalves et al. 2007). Meanwhile, Cu and Ni decrease their concentrations during the drought times.

The effect of climatic drought effect over the variations of (As) is evident in Fig. 3, the period before declaration of drought (years 2002) the concentrations of arsenic do not overpass the 15 µg/L, meanwhile in the drought period (2005–2008) the concentrations in a localized zone arrive to 80 µg/L in year 2005. The As concentrations are continuously increasing reaching 90 µg/L a in the year 2008. This situation changes in the years 2010 and 2011 when the rain is back, and the effect of the drought is not present, reducing the As concentration to 10 µg/L in the studied zone.

That aquifer behavior is a clear evidence of drought effects in the piezometric evolution; when the rain scarcity is present, the groundwater flow and volume decrease, increasing the periods of residence parallel to the concentration of As and reducing the area of influence (Devi et al. 2010; Gonçalves et al. 2007).

Conclusions

The period of drought in the years 2005–2008 was accumulated an important humidity deficit in Baix Ter aquifer, causing an episode of natural contamination of groundwater, which was manifested by an increase in arsenic concentration in the groundwater extracted from a small area near Fontanillas town on the NE of Catalunya. The hydrogeochemical analysis showed the geological origin of the arsenic presence in the groundwater of the area, basically associated with dissolution of oxides of arsenic from sediments that form the geology of Baix Ter aquifer.

This episode was a side effect of drought, and it is evidence of the parallel affectations of the depletion of the levels of groundwater over the hydrogeochemistry of aquifers, and how this affects the potential use of this hydrological resources.

Notes

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Authors and Affiliations

  • René Ventura-Houle
    • 2
    Email author
  • Xavier Font
    • 1
  • Lorenzo Heyer
    • 2
  1. 1.Geology FacultyUniversitat de BarcelonaBarcelonaSpain
  2. 2.Engineering and Science FacultyUniversidad Autónoma de TamaulipasCiudad VictoriaMexico

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